Electrochimica Acta, Journal Year: 2024, Volume and Issue: 484, P. 144048 - 144048
Published: March 4, 2024
Language: Английский
Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)
Published: April 9, 2024
The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the reduction reaction (ORR) kinetics. Herein, a new approach for boosting inherent ORR activity atomically dispersed Fe-N-C matrix is represented by implanting Fe atomic clusters nearby. as-prepared catalyst delivers excellent half-wave potentials 0.78 0.90 V in acidic alkaline solutions, respectively. decent can also be validated from high-performance rechargeable Zn-air battery. experiments density functional theory calculations reveal that electron spin-state monodispersed active transferred low spin (LS, t
Language: Английский
Citations
102
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)
Published: March 18, 2024
Abstract Recently, a diverse array of novel metal‐nitrogen‐carbon (M‐N‐C) single‐atom catalysts (SACs) have rapidly evolve, particularly in the realm oxygen reduction reaction (ORR). Despite plethora proposed design and improvement strategies for SACs, comprehensive review systematically compiling components M‐N‐C from unified perspective is notably absent. For first time, thorough examination each component conducted, focusing on entropy increase active sites SACs. single M‐N 4 whole system, an implies elevated degree disorder chaos. Broadly, entropy‐increasing modification M (single mental sites) guest groups entails augmentation chaos, with most effective co‐catalytic synergy achieved by establishing multiple through “cocktail effect”. Concerning N (nitrogen other heteroatoms) C (carbon supports), induces heightened disorder, symmetry breaking more likely to drive toward adsorbing molecules attain equilibrium symmetric structure. All these innovative led remarkable ORR activity stability offer guiding criterion future preparation
Language: Английский
Citations
27
Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 4847 - 4870
Published: Jan. 1, 2024
Based on the advancements in atomically dispersed multi-site catalysts for FZABs, this review discusses design methodologies to regulate performance of bifunctional oxygen electrocatalysts from electronic and geometric structures.
Language: Английский
Citations
23
Small, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 2, 2025
Abstract The dual‐site electrocatalysts formed by metal single atoms combines with nanoparticles represent a promising strategy to enhance both oxygen reduction reaction (ORR) and evolution (OER) performance. Herein, defect engineering is applied ORR OER electrocatalysts. Its design, synthesis, structural properties, catalytic performance experimentally theoretically are insightfully studied for the single‐atomic Fe─N 4 adjacent Fe 7 Co 3 nanoalloy (FeCo NA ) as loading on nitrogen‐doped graphene aerogel (Fe─N/FeCo@NGA). high‐density dual‐sites, together good electronic conductivity of NGA, synergistically improve structure superior electrocatalytic activity. half‐wave potential Fe─N/FeCo@NGA in 0.92 V overpotential it 1.58 V. Corresponding all‐solid‐state Zn‐air battery demonstrates peak power density 147.6 mW cm −2 charge/discharge durability over 140 h. Theoretical calculations reveal that Fe‐N FeCo skeleton optimized further refine local structure, modulating tensile force O─O bond * OOH intermediate, leading its spontaneous dissociation facilitating significantly reduced energy barrier. This work takes shortcut application development highly efficient bifunctional atoms.
Language: Английский
Citations
2
Small, Journal Year: 2023, Volume and Issue: 20(20)
Published: Dec. 10, 2023
Abstract The problem in d‐band center modulation of transition metal‐based catalysts for the rate‐determining steps oxygen conversion is an obstacle to boost electrocatalytic activity by accelerating proton coupling. Herein, Co doping FeP adopted modify Fe. Optimized Fe sites accelerate coupling reduction reaction (ORR) on N‐doped wood‐derived carbon through promoting water dissociation. In situ generated optimize adsorption oxygen‐related intermediates evolution (OER) CoFeP NPs. Superior catalytic toward ORR (half‐wave potential 0.88 V) and OER (overpotential 300 mV at 10 mA cm −2 ) express unprecedented level carbon‐based metal‐phosphide catalysts. liquid zinc–air battery presents outstanding cycling stability 800 h (2400 cycles). This research offers a newfangled perception designing highly efficient bifunctional OER.
Language: Английский
Citations
23
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Aug. 17, 2024
Abstract Iron‐based single‐atom catalysts (Fe─N─C) exhibit excellent oxygen reduction activity but struggle with bifunctional performance due to their poor evolution activity. Although the Fe spin state is found be closely associated enhanced activity, controllably regulating remains a challenge. Here, controllable regulation of directly achieved through competitive coordination between chlorine and pyridine nitrogen in axial direction Fe─N 4 . The regulated from high intermediate by modulation ligands weak‐field ligand strong‐field pyridinic nitrogen, which leads N─FeN small potential gap (Δ E = 0.68 V). Theoretical calculations indicate that turning accompanied an binding strength sites *OH leading significant decrease OER barrier. Moreover, exhibits sufficient durability for reaction (ORR) (over 50 h), (OER) 200 assembled zinc–air battery 1000 h). Here novel approach proposed designing efficient based on profound insights into Fe─N─C catalysis.
Language: Английский
Citations
10
Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 357, P. 124254 - 124254
Published: May 31, 2024
Language: Английский
Citations
9
Advanced Science, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 13, 2025
Abstract The cobalt‐nitrogen‐carbon (Co─N─C) single‐atom catalysts (SACs) are promising alternatives to precious metals for catalyzing the hydrogen evolution reaction (HER) and their activity is highly dependent on coordination environments of metal centers. Herein, a NaHCO 3 etching strategy developed introduce abundant in‐plane pores within carbon substrates that further enable construction low‐coordinated asymmetric Co─N sites with nearby vacancy defects in Co─N─C catalyst. This catalyst exhibits high HER an overpotential ( η ) merely 78 mV deliver current density 10 mA cm −2 , Tafel slope 45.2 dec −1 turnover frequency 1.67 s (at = 100 mV). Experimental investigations theoretical calculations demonstrate neighboring can modulate electronic structure alter adsorption configuration H intermediate from typical atop mode side mode, resulting weakened strength thus improved activity. work provides efficient regulate environment SACs catalytic performance sheds light atomic‐level understanding structure‐activity relationships.
Language: Английский
Citations
1
Nanomaterials, Journal Year: 2025, Volume and Issue: 15(2), P. 128 - 128
Published: Jan. 16, 2025
Zeolitic imidazolate framework-8 (ZIF-8) has been extensively studied as a precursor for nitrogen-doped carbon (NC) materials due to its high surface area, tunable porosity, and adjustable nitrogen content. However, the intrinsic microporous structure of ZIF-8 limits mass transport accessibility reactants active sites, reducing effectiveness in electrochemical applications. In this study, soft templating approach using triblock copolymer was used prepare mesoporous ZIF-8-derived NC (Meso-ZIF-NC) samples. The hierarchical porous investigated by varying ratios Pluronic F-127, NaClO4, toluene. resulting Meso-ZIF-NC exhibited widespread pore size distribution with an enhanced mesopore (2–50 nm) volume according composition reaction mixtures. Pt nanoparticles were uniformly dispersed on form Pt/Meso-ZIF-NC catalysts, which presented area improved oxygen reduction activity. study highlights important role doping enhancing catalytic performance, providing pathway advanced fuel cell catalyst design.
Language: Английский
Citations
1
Advanced Science, Journal Year: 2024, Volume and Issue: 11(39)
Published: Aug. 19, 2024
Abstract Single‐atom catalysts (SACs) with edge‐located metal active sites exhibit superior oxygen reduction reaction (ORR) performance due to their narrower energy gap and higher electron density. However, controllably designing such fully reveal advantages remains challenging. Herein, rich Fe‐N 4 anchored in hierarchically porous carbon nanofibers (denoted as e 1 ‐Fe‐N‐C) are fabricated via an situ zinc‐assisted thermal etching strategy. The ‐Fe‐N‐C catalyst demonstrates alkaline ORR activity compared counterparts fewer commercial Pt/C. Density functional theory calculations show that the accumulation of more negative charges near formation partially reduced Fe state reduce barrier for process. Additionally, unique structures mesopores macropores facilitate full utilization enhance long‐range mass transfer. zinc–air battery (ZAB) assembled has a peak power density 198.9 mW cm −2 , Pt/C (152.3 ). present strategy by facile controlling amount zinc acetate template systematically superiority sites, providing new design avenue rational defect engineering achieve high‐performance ORR.
Language: Английский
Citations
6